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Título

Pyridinethiolate titanocene metalloligands and their self-assembly reactions to yield early–late metallamacrocycles

AutorFerrer, Montserrat; Gómez-Bautista, Daniel ; Gutiérrez, Albert; Orduña-Marco, Guillermo; Oro, Luis A. ; Pérez-Torrente, Jesús J. ; Rossell, Oriol; Ruiz, Eliseo
Fecha de publicación2016
EditorAmerican Chemical Society
CitaciónOrganometallics 35 (3): 336-345 (2016)
ResumenNew titanocene pyridinethiolate compounds [(RCp)2Ti(4-Spy)2] (R = H (1), Me (2); Cp = cyclopentadienyl; 4-Spy = pyridine-4-thiolate) and [Cp2Ti(2-Spy)2] (3; 2-Spy = pyridine-2-thiolate) have been prepared by reaction of the corresponding Li(Spy) salt with the appropriate compound [(RCp)2TiCl2]. Compounds 1 and 2 have been used as metalloligands in self-assembly reactions with the acceptor late-transition-metal compounds [M(H2O)2(dppp)](OTf)2 (M = Pd (a) Pt (b); dppp = 1,3-bis(diphenylphosphino)propane), and the series of early–late tetranuclear metallamacrocycles [{(RCp)2Ti(4-Spy)2}{M(dppp)}]2(OTf)4 (R = H, M = Pd (12a2); R = H, M = Pt (12b2); R = Me, M = Pd (22a2); R = Me, M = Pt (22b2)) arising from the anti isomer of the titanocene metalloligands have been obtained. Only ligand transfer reactions from Ti to either Pd or Pt atoms have been observed when the pyridine-2-thiolate derivative 3 has been assayed in self-assembly processes. The obtained species have been characterized by NMR spectroscopy and ESI(+) mass spectrometry. The supramolecular assemblies have shown to be nonrigid in solution, and their fluxional behavior has been studied by VT 1H NMR spectroscopy. A DFT study including ab initio molecular dynamics in order to elucidate the structures and the relative stability of the isomers has been performed.
Versión del editorhttp://dx.doi.org/10.1021/acs.organomet.5b00876
URIhttp://hdl.handle.net/10261/133815
DOI10.1021/acs.organomet.5b00876
ISSN0276-7333
E-ISSN1520-6041
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